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功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理

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崔巍, 张卫, 刘淋, 温东东, 沈根祥, 胡双庆. 功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理[J]. 环境化学, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
引用本文: 崔巍, 张卫, 刘淋, 温东东, 沈根祥, 胡双庆. 功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理[J]. 环境化学, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
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CUI Wei, ZHANG Wei, LIU Lin, WEN Dongdong, SHEN Genxiang, HU Shuangqing. Adsorption behavior and mechanism of functional mental organic frameworks for sulfachloropyridazine in water[J]. Environmental Chemistry, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
Citation: CUI Wei, ZHANG Wei, LIU Lin, WEN Dongdong, SHEN Genxiang, HU Shuangqing. Adsorption behavior and mechanism of functional mental organic frameworks for sulfachloropyridazine in water[J]. Environmental Chemistry, 2020, (1): 80-88. doi: 10.7524/j.issn.0254-6108.2019012701
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功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理

  • 1. 华东理工大学资源与环境工程学院, 上海, 200237;

  • 2. 同济大学环境科学与工程学院, 上海, 200092;

  • 3. 上海市环境科学研究院, 上海, 200233

    • 通讯作者: 张卫, E-mail: wzhang@ecust.edu.cn ; 
  • 基金项目:

    国家"十三五"水体污染控制与治理科技重大专项（2017ZX07207002）和国家自然科学基金（41877124，21737005）资助.

Adsorption behavior and mechanism of functional mental organic frameworks for sulfachloropyridazine in water

  • 1. School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai, 200237, China;

  • 2. School of Environmental Science and Engineering, Tongji University, Shanghai, 200092, China;

  • 3. Shanghai Academy of Environmental Sciences, Shanghai, 200233, China

    • Corresponding author: ZHANG Wei, wzhang@ecust.edu.cn ; 
  • Fund Project: Supported by National Water Pollution Control and Treatment Science and Technology Major Project (2017ZX07207002) and the National Natural Science Foundation of China (41877124, 21737005).

  • 摘要: 近年来，抗生素的大量使用对生态环境和人类健康构成了严重威胁.抗生素去除技术开发引起了人们的广泛关注.本研究制备了4种具有良好水热稳定性的锆基金属骨架有机材料（UiO-66，UiO-66-NH2，UiO-66-Cl和UiO-66-NO2），通过比较4种材料对水中痕量磺胺氯哒嗪（SCP）的吸附性能，从中筛选出最佳吸附剂，进而探究了温度、pH、共存阴离子、腐殖酸和可再生性等因素对其吸附性能的影响，探讨了作用机制.研究结果表明，功能基团的引入提升了金属骨架有机材料对SCP的吸附性能，其中氨基的引入效果最为显著（去除率从11.62%提升至71.12%），这主要是由于氢键的作用；UiO-66-NH2对SCP的吸附符合拟二级动力学，温度的升高抑制了吸附的进行，pH=6时吸附效果最好；Cl-和SO42-对UiO-66-NH2吸附性能起到了抑制作用，而腐殖酸影响较小；CO32-的水解导致路易斯酸碱反应，从而极大地干扰了SCP的吸附过程；UiO-66-NH2经过四次循环使用后，SCP去除率下降不到10%.本研究为采用功能化金属有机骨架材料去除水中污染物提供了新思路.
    Abstract: In recent years, extensive use of antibiotics has greatly threatened the ecological environment and human health, so the removal of antibiotics has been widely investigated. In this study, four zirconium-based metal organic framework (MOF) materials (UiO-66, UiO-66-NH2, UiO-66-Cl and UiO-66-NO2) with good hydrothermal stability were synthesized to compare their adsorption performance in removing sulfachloropyridazine (SCP) from water. The effects of temperature, pH, coexisting anion, and humic acid on the adsorption performance of the optimal material were explored. The results show that the introduction of functional groups into MOF enhanced the adsorption ability of UiO-66 for SCP, and the effect of amino group was the most significant (SCP removal rate increased from 11.62% to 71.12%), which might be due to hydrogen bonding. The adsorption of SCP by UiO-66-NH2 accorded with the pseudo-second order kinetics model, and the adsorption process was inhibited at high temperatures. Co-existing anions including Cl-, SO42- and CO32- reduced the adsorption ability, and the presence of CO32- inhibited the adsorption process the most because of the Lewis acid-base reaction. Humic acid had no influences on the adsorption performance of UiO-66-NH2, and the removal efficiency of UiO-66-NH2 decreased by less than 10% after four cycles of use. This study provides a new idea for using functionalized metal-organic framework materials to remove contaminants in water body.
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  • 收稿日期:  2019-01-27
  • 刊出日期:  2020-01-01

功能化金属有机骨架材料对水中痕量磺胺氯哒嗪的吸附行为及其机理

    通讯作者: 张卫, E-mail: wzhang@ecust.edu.cn ; 
  • 1. 华东理工大学资源与环境工程学院, 上海, 200237;
  • 2. 同济大学环境科学与工程学院, 上海, 200092;
  • 3. 上海市环境科学研究院, 上海, 200233
  • 收稿日期:  2019-01-27
  • 网络出版日期:  2020-01-01
基金项目:

国家"十三五"水体污染控制与治理科技重大专项（2017ZX07207002）和国家自然科学基金（41877124，21737005）资助.

摘要: 近年来，抗生素的大量使用对生态环境和人类健康构成了严重威胁.抗生素去除技术开发引起了人们的广泛关注.本研究制备了4种具有良好水热稳定性的锆基金属骨架有机材料（UiO-66，UiO-66-NH2，UiO-66-Cl和UiO-66-NO2），通过比较4种材料对水中痕量磺胺氯哒嗪（SCP）的吸附性能，从中筛选出最佳吸附剂，进而探究了温度、pH、共存阴离子、腐殖酸和可再生性等因素对其吸附性能的影响，探讨了作用机制.研究结果表明，功能基团的引入提升了金属骨架有机材料对SCP的吸附性能，其中氨基的引入效果最为显著（去除率从11.62%提升至71.12%），这主要是由于氢键的作用；UiO-66-NH2对SCP的吸附符合拟二级动力学，温度的升高抑制了吸附的进行，pH=6时吸附效果最好；Cl-和SO42-对UiO-66-NH2吸附性能起到了抑制作用，而腐殖酸影响较小；CO32-的水解导致路易斯酸碱反应，从而极大地干扰了SCP的吸附过程；UiO-66-NH2经过四次循环使用后，SCP去除率下降不到10%.本研究为采用功能化金属有机骨架材料去除水中污染物提供了新思路.

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